Bacterial cellulose (BC) is a green biopolymer suitable for heavy metal ion removal from aqueous solution due to its nano-porous microstructure. Polyethyleneimine-bacterial cellulose (PEI-BC) was prepared by reductive amination of dialdehyde BC with polyethyleneimine. The capacity of PEI-BC in Cu(II) and Pb(II) adsorption from aqueous solution was investigated. The adsorption kinetics could be well expressed by pseudo-second-order model and the adsorption isotherm data were well fitted with Freundlich model. Adsorption processes of Cu(II) and Pb(II) by PEI-BC reached equilibrium very rapid in 30 and 60 min, respectively. The maximum adsorption capacity of PEI-BC on Cu(II) and Pb(II) was found to be 148 and 141 mg/g, respectively, which was higher than that of unmodified BC and other modified BC reported. PEI-BC also showed good reusability in the adsorption of Cu(II) and Pb(II). This study demonstrates that polyethyleneimine modification makes BC a potential bioadsorbent for heavy metal ion removal in waste water.